Vesosomes are nested liposomal structures with high potential as advanced drug delivery vehicles, bioreactors and artificial cells. However, to date no method has been reported prepare monodisperse vesosomes of controlled size. Here we report on a multistep microfluidic strategy for hierarchically assembling uniform from dewetting double emulsion templates. The control afforded by our is illustrated the formation concentric, pericentric multicompartment liposomes. route offers an exceptional...

Abstract Hydrogels have been designed to react many different stimuli which find broad applications in tissue engineering and soft robotics. However, polymer networks bearing mechano-responsiveness, especially those displaying on-demand self-stiffening self-softening behavior, are rarely reported. Here, we design a mechano-controlled biocatalytic system at the molecular level that is incorporated into hydrogels regulate their mechanical properties material scale. The consists of protease...

The compartmentalization of cell-free gene expression systems in liposomes provides an attractive route to the formation protocells, but these models do not capture physical (crowded) environment found living systems. Here, we present a microfluidics-based produce monodisperse that can shrink almost 3 orders magnitude without compromising their stability. We demonstrate our strategy is compatible with and show increased protein production rates crowded liposome protocells.

DNA-incorporating hydrophobic moieties can be synthesized by either solid-phase or solution-phase coupling. On a solid support the DNA is protected, and units are usually attached employing phosphoramidite chemistry involving synthesizer. other hand, solution coupling in aqueous medium results low yields due to solvent incompatibility of compounds. Hence, development general method for producing amphiphilic conjugates with high yield remains major challenge. Here, we report an organic-phase...

Significance Liquid crystals (LCs) found in biology are usually dispersed a solvent, typically water, and therefore classified as lyotropic. However, from technological perspective, thermotropic LCs (TLCs), based on small rod- or disc-shaped organic molecules, have been of much greater importance. In this contribution, we show that liquid crystal phases materials can also be made biomolecules, demonstrating simple generic method to form biosystems ranging nucleic acids proteins even whole...

Abstract Chiral macromolecules have been widely used as synthetic pockets to mimic natural enzymes and promote asymmetric reactions. An achiral host, cucurbit[8]uril (CB[8]), was for an Lewis acid catalyzed Diels–Alder reaction. We achieved a remarkable increase in enantioselectivity large rate acceleration the presence of nanoreactor by using amino chiral source. Mechanistic computational studies revealed that both acid–Cu 2+ complex dienophile substrate are included inside macrocyclic host...

Abstract Deoxyribonucleic acid (DNA) represents an important class of molecular building blocks for the assembly supramolecular functional systems primarily due to its recognition capability and sequence programmability. Eventually, DNA‐based nanostructures are assembled in a way that their states remain at thermodynamic minimum energy. However, active life‐like functions interactive adaption require integration energy away from equilibrium. The construction artificial was often inspired by...

Polymer mechanochemistry is a promising technology to convert mechanical energy into chemical functionality by breaking covalent and supramolecular bonds site-selectively. Yet, the mechanochemical reaction rates of in typically used ultrasonication setups lead reasonable conversions only after comparably long sonication times. This can be accelerated either increasing reactivity mechanoresponsive moiety or modifying encompassing polymer topology. Here, microbubble system with tailored shell...

Abstract Organization of gold nanoobjects by oligonucleotides has resulted in many three‐dimensional colloidal assemblies with diverse size, shape, and complexity; nonetheless, autonomous temporal control during formation remains challenging. In contrast, living systems temporally spatially self‐regulate functional structures internally orchestrating assembly disassembly kinetics dissipative biomacromolecular networks. We present a novel approach for fabricating four‐dimensional...

Abstract Herein, we present the divergent syntheses of α‐arylacylamides and oxindoles via mechanoredox chemistry by using easily accessible α‐bromo N ‐sulfonyl amides as starting materials. Our system consists a catalytic amount Cu II precatalyst piezoelectric The highly polarized BaTiO 3 or PbTiO under mechanical agitation can act an electron donor to realize recycling I . Control experiments density functional theory calculations have been performed support proposed mechanistic rationale...

Abstract Protein self‐assembly allows for the formation of diverse supramolecular materials from relatively simple building blocks. In this study, a single‐component self‐assembling hydrogel is developed using recombinant protein CsgA, and its successful application spinal cord injury repair demonstrated. Gelation achieved by physical entanglement CsgA nanofibrils, resulting in self‐supporting at low concentrations (≥5 mg mL −1 ). By leveraging programmability gene sequence, bioactive...

Abstract A traumatic tissue adhesive technology is highly sought after in ophthalmic surgery; however, many polymeric adhesives face significant limitations clinical ophthalmology, particularly corneal transplantation. major challenge achieving rapid adhesion without introducing polymer barriers or chemical toxicity from cross-linking. To address this, we developed a novel cornea-specific nanoadhesive constructed through protein-DNA co-assembly and applied it to In this system, rigid...

Herein, metal-organic frameworks UiO-66 and UiO-66-NH2 were synthesized, their piezoelectric properties characterized by piezoresponse force microscopy. Under mechanical agitation, the highly polarized can act as electron donors to reduce aryl diazonium salts, forming radical species, which further react with bis(pinacolato)diborane or heteroarenes generate desired products broad substrate scope. For all substrates, it was found that reactions mediated , exhibited better property, more...

Glues are being used to bond, seal, and repair in industry biomedicine. The improvement of gluing performance is hence important for the development new glues with better balanced property spaces, which turn necessitates a mechanistic understanding their mechanical failure. Optical force probes (OFPs) allow observation material damage polymers from macro- down microscale, yet have never been employed glues. Here, series ratiometric OFPs based on fluorescent-protein-dye protein-protein...

Abstract Cyclic peptides containing a disulfide bridge were identified as simple and versatile coordination sphere for asymmetric catalysis. Upon complexation with Cu 2+ ions they catalyze Diels–Alder Friedel–Crafts reactions high enantioselectivities of up to 99 % ee 86 , respectively. Moreover, the ligands systematically optimized assistance “Alanine Scanning”. This biomolecular design could greatly expand choice peptide scaffolds artificial metallopeptide catalysts.

Protein crystallization is an important tool for structural biology and nanostructure preparation. Here, we report on kinetic pathway-dependent protein crystals that are controlled by light. Photo-responsive crystallites obtained complexing the model proteins with cationic azobenzene dyes. The crystalline state readily switched to a dispersed phase under ultraviolet light restored subsequent visible-light illumination. switching can be reversibly repeated multiple cycles without noticeable...

The ultrasound (US)‐induced activation of mechanophores embedded in linear polymers (LPs) is the most widely employed technique to realize chemical function by polymer mechanochemistry. However, commonly used US frequency this context around 20 kHz, producing strong inertial cavitation limiting biomedical applicability. Herein, kHz and 1.5 MHz high‐intensity focused (HIFU) are investigated drive disulfide mechanophore mechanochemical chain scission network core‐structured star (NCSPs). It...

Abstract Chiral macromolecules have been widely used as synthetic pockets to mimic natural enzymes and promote asymmetric reactions. An achiral host, cucurbit[8]uril (CB[8]), was for an Lewis acid catalyzed Diels–Alder reaction. We achieved a remarkable increase in enantioselectivity large rate acceleration the presence of nanoreactor by using amino chiral source. Mechanistic computational studies revealed that both acid–Cu 2+ complex dienophile substrate are included inside macrocyclic host...

Herein, we present a DNA circuit programmed for the delivery of CpG oligodeoxynucleotides (CpG ODNs) with pharmacological immunostimulation function. The employs complementary (cDNA) strand to deactivate biological function ODNs via hybridization, while T7 exonuclease mediates activation by hydrolyzing cDNA and releasing ODN as an active moiety. We investigated influence several factors on kinetic profile temporal behavior circuit. These include design strand, concentration duplex,...

Metal nanoparticles exhibit unique size- and spatial organization-dependent physical chemical properties, have a wide range of applications in various areas including single electron devices, catalysts biomedicines. In this paper, chains palladium were obtained by incubating aged sodium tetrachloropalladate(II) with glucagon fibrils pre-deposited on solid surface. AFM height profiles showed that the size within could be fine tuned ∼2 to 16 nm as function concentration...